Platinum group metal(PGM)electrocatalysts play an irreplaceable role in many electrochemical reactions for sustainable energy conversion.In the past few decades,the electronic orbital modulation methods have emerged a...Platinum group metal(PGM)electrocatalysts play an irreplaceable role in many electrochemical reactions for sustainable energy conversion.In the past few decades,the electronic orbital modulation methods have emerged as an important way to produce high-performance electrocatalysts,often by adjusting surface reactivity and enhancing structural stability.In this review,we first systematically elaborate on the basic principles and stra-tegies of orbital modulation for PGM-based catalysts,mainly from the perspective of improving activity and stability,in which we highlight some exploratory theoretical studies over the past few decades.Then we describe a series of representative works to elucidate the specific approaches used to realize precise orbital modulation in PGM catalysts.Finally,we clarify the existing challenges and propose some perspectives for the development of related theories and practical applications.展开更多
Solid-state lithium battery(SSLB)is considered as one of the promising candidates for next-generation power batteries due to high safety,unprecedented energy density and favorable adaptability to high pression and tem...Solid-state lithium battery(SSLB)is considered as one of the promising candidates for next-generation power batteries due to high safety,unprecedented energy density and favorable adaptability to high pression and temperature.However,the system of solid electrolyte(SE),as one of the most important components in SSLB,is usually plagued by clumsy ionic transport,leading to poor rate performance of the SSLBs.Herein,a unique perspective is proposed to re-examine the ion-transport behavior in lithium conductors by tracing Liþat multiscale,including microscopic,mesoscopic and macroscopic scales.The multi-scale ion-transport mechanisms and corresponding characterization techniques are analyzed in depth.Furthermore,some strategies of structure design to improve ion-transport kinetics at corresponding scales are elaborated systematically,involving the modulation of microscopic homogeneous structure,mesoscopic heterogeneous structure and macroscopic structures,etc.The proposed generalized rules for SEs are expected to construct a close link from mechanism-structure-characterization to high performances for SSLBs.展开更多
Stabilizing the highly active RuO_(2) electrocatalyst for the oxygen evolution reaction(OER)is critical for the application of proton exchange membrane water electrolysis,but this remains challenging due to the inevit...Stabilizing the highly active RuO_(2) electrocatalyst for the oxygen evolution reaction(OER)is critical for the application of proton exchange membrane water electrolysis,but this remains challenging due to the inevitable over-oxidation of Ru in harsh oxidative environments.Herein,we describe constructing Ru-O-La asymmetric configurations into RuO_(2) via a facile sol-gel method to tailor electron redistribution and thereby eliminate the over-oxidation of Ru centers.Specifically,the as-prepared optimal La_(0.1)Ru_(0.9)O_(2) shows a low overpotential of 188 mV at 10 mA cm^(-2),a high mass activity of 251 A gRu^(-1) at 1.6 V vs.reversible hydrogen electrode(RHE),and a long-lasting durability of 63 h,far superior to the 8 h achieved by standard RuO_(2).Experiments and density functional theory calculations jointly reveal that the Ru-O-La asymmetric configuration could trigger electron redistribution in RuO_(2).More importantly,electron transfer from La to Ru via the Ru-O-La configuration could lead to increased electron density around Ru,thus preventing the over-oxidation of Ru.In addition,electron redistribution tunes the Ru 4d band center’s energy level,which optimizes the adsorption and desorption of oxygen intermediates.This work offers an effective strategy for regulating electronic structure to synergistically boost the activity and stability of RuO_(2)-based acidic OER electrocatalysts.展开更多
Aqueous zinc-ion batteries(ZIBs)represent a promising solution for“beyond-lithium-ion”chemistries,but certain problems hinder their further development,especially when conventional aqueous electrolytes are involved....Aqueous zinc-ion batteries(ZIBs)represent a promising solution for“beyond-lithium-ion”chemistries,but certain problems hinder their further development,especially when conventional aqueous electrolytes are involved.Hydrogel polymer electrolytes(HPEs)offer opportunities to circumvent these issues.This review aims to provide a fundamental understanding of how to design better HPEs for high-performing ZIBs,through critically analyzing the recent literature.Concerns regarding HPEs’mechanical,interfacial,and electrochemical characteristics are addressed,followed by in-depth insights into their underlying mechanisms.Possibilities for practical applications of HPEs are also discussed.展开更多
As an important component in electrochemical energy conversion and storage systems,electrochemical reactors(ECRs)are widely used for commodity chemical synthesis,including electrolytic H_(2)production,NH_(3)synthesis,...As an important component in electrochemical energy conversion and storage systems,electrochemical reactors(ECRs)are widely used for commodity chemical synthesis,including electrolytic H_(2)production,NH_(3)synthesis,and high-value CO_(2)utilization.However,ECRs pose challenges related to low energy efficiency and selectivity due to the low solubility of their gaseous reactants,slow kinetics,and limitations in mass transfer.It is thus imperative to develop advanced high-pressure(HP)ECRs to address these issues.In this review,we start by presenting a comprehensive analysis of the fundamental mechanisms of HP ECRs.Then,we summarize the stateof-the-art HP ECR applications for water electrolysis,the N_(2)reduction reaction,and the CO_(2)reduction reaction.We also demonstrate that mathematical simulations are valuable tools for digital validation and guidance to accelerate the design of better reactors.Finally,we make recommendations on developing relevant specifications and standards for the industrial application of HP ECRs.展开更多
There is an urgent need to develop innovative electrochemical energy storage devices that can offer high energy density,long lifespan,excellent rate capability,and improved security.For the electrochemical system,the ...There is an urgent need to develop innovative electrochemical energy storage devices that can offer high energy density,long lifespan,excellent rate capability,and improved security.For the electrochemical system,the electrode interphase,namely the cathode electrolyte interphase(CEI)and solid electrolyte interphase(SEI)play crucial roles in the operating mechanism,kinetics,and overall performance of the battery.However,the in-depth investigation of the unstable and complex electrode interphase is limited by the unavoidable air and moisture contact during the material transfer process and probable high-energy radiation damage in the characterization procedure.Recently,cryogenic techniques and in situ techniques have been developed and applied in the electrode interphase research to settle the radiation damage and air erosion,respectively.However,there has not been a special review that summarizes the relevant methods,so a systematic review is very important to accelerate the development.In this review,we summarize these two state-of-the-art methods,including their working principle,characterization process,advantages,and applications in electrode interphase analysis.And the integrative techniques,which are considered as the future development perspectives,are also discussed.This review can provide important directions for next-generation characterization techniques and strategies to effectively analyze the electrode interphase for advanced batteries.展开更多
Electrochemical water splitting is a pivotal technology in the large-scale production of green hydrogen for sus-tainable future energy provisions.Highly active,stable electrocatalysts have been extensively explored,bu...Electrochemical water splitting is a pivotal technology in the large-scale production of green hydrogen for sus-tainable future energy provisions.Highly active,stable electrocatalysts have been extensively explored,but the majority suffer from low current densities and small sizes,rendering them unsuitable for industrial applications.Recently,however,the scalable production of electrocatalysts with high performance at large current densities has made tremendous progress.In this review,the current achievements in developing outstanding large elec-trocatalysts for high-current-density water electrolysis are described in detail.First,we introduce the funda-mentals of water electrolysis,the criteria for performance evaluation,and the requirements for producing electrocatalysts at scale under large current densities.Second,we summarize the key approaches for realizing large-sized electrocatalysts with excellent performance,including electrodeposition,corrosion engineering,and thermal treatment,as well as combinations of these methods.Finally,we offer perspectives on research challenges and propose directions for mass-producing high-performance electrocatalysts with large current densities for water electrolysis,to guide the further industrialization of water-electrolysis catalysts.展开更多
Interfacial H_(2)release severely limits the reversibility and feasibility of aqueous Zn metal batteries for large-scale energy storage.Different from the conventional perception that H_(2)release mainly originates fr...Interfacial H_(2)release severely limits the reversibility and feasibility of aqueous Zn metal batteries for large-scale energy storage.Different from the conventional perception that H_(2)release mainly originates from the competition between hydrogen evolution reaction and Zn plating process,we herein surprisingly find that non-negligible H_(2)is also generated during stripping due to the accelerated chemical corrosion of the newly exposed Zn surface.To address this issue,we systematically screened the organic additives with different molecular structures and functional groups.Interestingly,a positive correlation between the adsorption strength of additives and the ability to inhibit the interfacial hydrogen release is found.Taking cysteamine(MEA)as a model additive,a gradient solid electrolyte interphase(SEI)is in situ formed at the Zn surface,acting as a chemical“barrier”to isolate interfacial water molecules from electrode surface consequently enable a higher Coulombic efficiency(>99.5%,4000 cycles)compared with that of MEA-free electrolyte(98.1%,189 cycles).This work provides a new understanding of the interfacial hydrogen release mechanism and the criteria for selecting additives for aqueous Zn metal anodes.展开更多
The application of electrochemical technologies for chemical and fuel synthesis offers a significantly more eco-friendly method than traditional industrial practice.However,electrochemical synthesis in aqueous solutio...The application of electrochemical technologies for chemical and fuel synthesis offers a significantly more eco-friendly method than traditional industrial practice.However,electrochemical synthesis in aqueous solutions often involves a sluggish oxygen evolution reaction(OER)at the anode,yielding products that are less economically viable and leading to inefficient energy use.This challenge has prompted extensive research into replacing the OER with fast,value-added oxidation reactions(OER alternatives)in electrolysis systems.In this review,we summarize the latest research progress in coupled electrochemical systems that integrate OER al-ternatives with reduction reactions,beyond hydrogen evolution reactions,in aqueous solutions to synthesize dual value-added products.After providing a general overview,we start by introducing two key factors:(i)electrolytic devices and(ii)advanced characterization techniques for mechanism investigation.The focus then shifts to catalysts developed so far and their corresponding catalytic mechanisms,and to the electrochemical performance of these hybrid electrolysis systems.Finally,we outline and discuss the challenges and prospects for these inte-grated electrochemical systems to offer insights into future research directions and applications.We envision that this review will provide a panorama of electrolysis systems for dual value-added products,thereby fostering the development of green synthesis with zero carbon emissions.展开更多
Building highly reactive electrocatalysts is of great significance for addressing the energy crisis and developing green energy.Electrocatalytic reactions occur at the interface of catalysts,where the physicochemical ...Building highly reactive electrocatalysts is of great significance for addressing the energy crisis and developing green energy.Electrocatalytic reactions occur at the interface of catalysts,where the physicochemical properties of the catalyst surface play a dominant role.In particular,the electron spin behavior on the catalyst surface has a decisive impact on the catalytic reaction process.This review initially introduces the definition of electron spin and methods for spin manipulation.Furthermore,we summarize the advanced characterization methods of electron spin.Then,we review the latest research advancements on the spin effect in the oxygen reduction reaction,oxygen evolution reaction,carbon dioxide reduction reaction,and nitrogen reduction reaction.The catalytic mechanisms of spin manipulation in these four reactions are thoroughly discussed.Finally,we propose key directions for the future development of spin effects in the field of electrocatalysis.This review contributes to a deeper understanding of the micromechanisms in electrocatalytic reactions.展开更多
It is anticipated that alkaline water electrolysis(AWE)technology will assume a significant role in the future energy sector,facilitating the integration of renewable energy and hydrogen production.Regrettably,the eff...It is anticipated that alkaline water electrolysis(AWE)technology will assume a significant role in the future energy sector,facilitating the integration of renewable energy and hydrogen production.Regrettably,the effi-ciency of AWE is not yet optimal.In particular,the inefficiency caused by bubbles at increased current density is often overlooked,necessitating a detailed understanding of the intricate relationship between bubble evolution and electrolytic reactions.This paper presents a comprehensive review of the fundamental theory and recent research on bubbles,and outlines the primary challenges and research directions for bubble dynamics in AWE.First,the theory of bubble nucleation,growth,and detachment is reviewed and summarized.Subsequently,the impact of bubbles on the diverse processes occurring during the electrolysis reaction is meticulously delineated and examined.The following section presents a thorough compilation and categorization of the methods employed to remove bubbles,with a detailed analysis of the strategies deployed to mitigate the impact of gas bubble traffic.Additionally,an in-depth exploration of the research methodology employed at each stage of the bubble evolution process is provided.Finally,the review concludes with a summary and outlook on the oppor-tunities and challenges associated with studying bubble dynamics in AWE,offering insights into innovative av-enues for efficient electrolytic hydrogen production.展开更多
The authors regret an inadvertent error in Fig.3a where a methyl group was drawn as an ethyl group in the trimethyl phosphate(TMP)structure,resulting in ethyl dimethylphosphate.This unintentional oversight occurred du...The authors regret an inadvertent error in Fig.3a where a methyl group was drawn as an ethyl group in the trimethyl phosphate(TMP)structure,resulting in ethyl dimethylphosphate.This unintentional oversight occurred during graphic preparation.A revised structure is provided here.展开更多
With issues of energy security and environmental crisis intensifying,we urgently need to develop energy storage systems with high energy density and high safety.Zinc–air batteries have attracted extensive attention f...With issues of energy security and environmental crisis intensifying,we urgently need to develop energy storage systems with high energy density and high safety.Zinc–air batteries have attracted extensive attention for their energy density,safety,and low cost,but problems with the zinc anode—such as hydrogen evolution,corrosion,passivation,dendrite proliferation,and deformation—have led to zinc–air batteries with low Coulombic efficiency and short cycle life;these remain the key obstacles hindering the batteries’further development.In this review paper,we briefly describe the reaction mechanism of zinc–air batteries,then summarize the strategies for solving the key issues in zinc anodes.These approaches are divided into three aspects:structural designs for the zinc anode;interface engineering;and electrolyte selection and optimization.We finish by offering some suggestions for future research directions to improve the zinc anode in zinc–air batteries.展开更多
The integration of surface plasmons with catalysis has opened a new frontier in the field of chemical energy conversion,offering unprecedented opportunities for enhancing reaction activity and selectivity.This review ...The integration of surface plasmons with catalysis has opened a new frontier in the field of chemical energy conversion,offering unprecedented opportunities for enhancing reaction activity and selectivity.This review delves into the optical properties of plasmonic materials,the intricate mechanisms of plasmon-assisted chemical reactions(PACRs),and the fabrication of plasmonic catalysts,highlighting the significance of the structure–performance relationship.The mechanisms of PACRs are summarized to understand their synergistic contributions to reactions.The review further examines modern experimental strategies for characterizing surface plasmon resonance properties,including scanning probe microscope,in situ spectroscopy,and ultrafast laser pump-probe techniques,which provide real-time,dynamic insights into molecular interactions and structural changes with high spatial and temporal resolution.We conclude by outlining the challenges and future prospects for PACRs,emphasizing the need for innovative strategies to fully exploit the potential of PACRs for sustainable energy conversion and environmental remediation.展开更多
Integrating single atoms and clusters into a unified catalytic system represents a novel strategy for enhancing catalytic performance.Compared to single-atom catalysts,those incorporating both single atoms and cluster...Integrating single atoms and clusters into a unified catalytic system represents a novel strategy for enhancing catalytic performance.Compared to single-atom catalysts,those incorporating both single atoms and clusters exhibit superior catalytic activity.However,the co-construction of these systems and the mechanisms of their catalytic efficacy remain challenging and poorly understood.In this study,we synthesized a Mn–N–C catalyst featuring MnY clusters and Mn single atoms via a straightforward two-step sintering method.Y doping facilitated the formation of Mn clusters and optimized the d-band center of Mn through a unique synergy effect,thereby reducing energy barriers and enhancing the reaction kinetics.Additionally,the electron-donating ability of Y single atoms promoted the formation of unsaturated Mn–N_(₃)coordination structures,resulting in excellent oxygen reduction reaction(ORR)performance.Consequently,the MnY/NC catalyst demonstrated a half-wave potential(E_(₁/₂))of 0.90 V and maintained stability in 0.1 M KOH,outperforming both Mn/NC and Pt/C.This work underscores the potential of rare earth metal doping in transition metals to create stable single-atom and cluster systems,effectively leveraging their synergy effect for superior catalytic performance and validating the concept of the“remote synergy effect”in heterogeneous catalysis.展开更多
Bismuth vanadate(BiVO_(4))is a promising photoanode material for photoelectrochemical(PEC)water oxidation.However,its performance is greatly hindered by poor bulk and interfacial charge transfer.Herein,to address this...Bismuth vanadate(BiVO_(4))is a promising photoanode material for photoelectrochemical(PEC)water oxidation.However,its performance is greatly hindered by poor bulk and interfacial charge transfer.Herein,to address this issue,iron doped vanadyl phosphate(Fe:VOPO_(4))was grafted on molybdenum doped BiVO_(4)(Mo:BiVO_(4))for significantly enhancing charge transfer and oxygen evolution kinetics simultaneously.Consequently,the resultant Fe:VOPO_(4)/Mo:BVO_(4) photoanode exhibits a remarkable photocurrent density of 6.59 mA cm^(-2) at 1.23 V versus the reversible hydrogen electrode(VRHE)under AM 1.5G illumination,over approximately 5.5 times as high as that of pristine BiVO_(4).Systematic studies have demonstrated that the hopping activation energy of small polarons is significantly reduced due to the Mo doping,resulting in accelerated bulk charge transfer.More importantly,the deposition of Fe:VOPO_(4) promotes the interfacial charge transfer between Mo:BiVO_(4) and Fe:VOPO_(4) via the construction of V-O-V and P-O bonds,in addition to facilitating water splitting kinetics.This work provides a general strategy for optimizing charge transfer process,especially at the interface between photoanodes and cocatalysts.展开更多
Black phosphorus(BP)anode with high capacity(2596 mAh g^(-1))and suitable lithiation potential(0.7 V vs.Li^(+)/Li)is an ideal candidate for high-energy-density and high-safety lithium-ion batteries,however,the practic...Black phosphorus(BP)anode with high capacity(2596 mAh g^(-1))and suitable lithiation potential(0.7 V vs.Li^(+)/Li)is an ideal candidate for high-energy-density and high-safety lithium-ion batteries,however,the practical implementation is greatly limited by its slow reaction kinetics and huge volume expansion.Here,inspired by nature,liquid metal(LM)is explored as a self-heal agent,which can well stabilize the BP anode through buffering the volumetric expansion and re-activating“dead P and Li x P”.Moreover,LM also acts as a good catalyst,which can adjust Li ion concentration and reduce the activation energy of delithiation reaction,thus prolonging the cycling life.Therefore,the LM modified BP/graphite(G)composite delivers an excellent high-rate performance of 1123 mAh g^(-1)at 4 C with 80.0%capacity retention after 200 cycles,a superior wide-temperature performance of 1547.5 mAh g^(-1)and 569.0 mAh g^(-1)at 50℃and-20℃,respectively.展开更多
Full-body avatar reconstruction offers users immersive and interactive experiences in virtual space,which are crucial for the advancement of metaverse applications.However,traditional hardware solutions,reliant on opt...Full-body avatar reconstruction offers users immersive and interactive experiences in virtual space,which are crucial for the advancement of metaverse applications.However,traditional hardware solutions,reliant on optical cameras or inertial sensors,are hampered by privacy concerns,spatial limitations,high costs,and calibration challenges.Here,we propose AI-enabled smart clothing that seamlessly integrates triboelectric strain-sensing fibers(TSSFs)and AI algorithms with commercial fitness suits to achieve precise dynamic 3D reconstruction of body movement.TSSFs enable the dynamic capture of body postures and excel in sensitivity,linearity,and strain range,while maintaining mechanical stability,temperature resilience,and washability.The integrated algorithms accurately decouple posture signals—distinguishing between similar postures with the 1D-CNN algorithm,compensating for body-shape differences via a calibration algorithm,and determining spatial elements for avatar reconstruction using a decision-tree algorithm.Finally,leveraging Unity-3D,we achieve ultra-accurate dynamic 3D avatars with a joint angle error of<3.63°and demonstrate their effectiveness using VR fitness and enter-tainment applications,showing how they can offer users standardized yet engaging experiences.展开更多
The Li-O_(2) battery(LOB)has attracted growing interest,including for its great potential in next-generation energy storage systems due to its extremely high theoretical specific capacity.However,a series of challenge...The Li-O_(2) battery(LOB)has attracted growing interest,including for its great potential in next-generation energy storage systems due to its extremely high theoretical specific capacity.However,a series of challenges have seriously hindered LOB development,such as sluggish kinetics during the oxygen reduction and oxygen evolution reactions(ORR/OER)at the cathode,the formation of lithium dendrites,and undesirable corrosion at the lithium metal anode.Herein,we propose a strategy based on the ultra-low loading of atomic Ni catalysts to simultaneously boost the ORR/OER at the cathode while stabilizing the Li metal anode.The resultant LOB delivers a superior discharge capacity(>16,000 mAh g^(-1)),excellent long-term cycling stability(>200 cycles),and enhanced high rate capability(>300 cycles@500 mA g^(-1)).The working mechanisms of these atomic Ni catalysts are revealed through carefully designed in situ experiments and theoretical calculations.This work provides a novel research paradigm for designing high-performance LOBs that are useable in practical applications.展开更多
Accelerated and accurate degradation diagnosis is imperative for the management and reutilization of commercial lithium-ion batteries in the upcoming TWh era.Different from traditional methods,this work proposes a hyb...Accelerated and accurate degradation diagnosis is imperative for the management and reutilization of commercial lithium-ion batteries in the upcoming TWh era.Different from traditional methods,this work proposes a hybrid framework for rapid and accurate degradation diagnosis at the electrode level combining both deep learning,which is used to rapidly and robustly predict polarization-free incremental capacity analysis(ICA)curves in minutes,and physical modeling,which is used to quantitatively reveal the electrode-level degradation modes by decoupling them from the ICA curves.Only measured charging current and voltage signals are used.Results demonstrates that 11 points collected at any starting state-of-charge(SOC)in a minimum of 2.5 minutes are sufficient to obtain reliable ICA curves with a mean root mean square error(RMSE)of 0.2774 Ah/V.Accordingly,battery status can be accurately elevated based on their degradation at both macro and electrode levels.Through transfer learning,such a method can also be adapted to different battery chemistries,indicating the enticing potential for wide applications.展开更多
基金supported by National Natural Science Foundation of China(22122202,21972051)Fundamental Research Funds for the Central Universities(No.YCJJ20230101).
文摘Platinum group metal(PGM)electrocatalysts play an irreplaceable role in many electrochemical reactions for sustainable energy conversion.In the past few decades,the electronic orbital modulation methods have emerged as an important way to produce high-performance electrocatalysts,often by adjusting surface reactivity and enhancing structural stability.In this review,we first systematically elaborate on the basic principles and stra-tegies of orbital modulation for PGM-based catalysts,mainly from the perspective of improving activity and stability,in which we highlight some exploratory theoretical studies over the past few decades.Then we describe a series of representative works to elucidate the specific approaches used to realize precise orbital modulation in PGM catalysts.Finally,we clarify the existing challenges and propose some perspectives for the development of related theories and practical applications.
基金supported by the Ministry of Science and Technology of the People's Republic of China(2022YFB2402200 and 2019YFA0705600)the National Natural Science Foundation of China(22121005,22005155,52072186,52203066,51673148 and 51678411)+5 种基金the Fundamental Research Funds for the Central Universities of China(63233017,63231002 and 63231198)the Science and Technology Plans of Tianjin,China(19PTSYJC00010)the China Postdoctoral Science Foundation Grant(2023M742135)the National Innovation and Entrepreneurship Training Program for College Students,China(202110058017)Tianjin Natural Science Foundation(23JCYBJC00660)Tianjin Enterprise Science and Technology Commissioner Project(23YDTPJC00490).
文摘Solid-state lithium battery(SSLB)is considered as one of the promising candidates for next-generation power batteries due to high safety,unprecedented energy density and favorable adaptability to high pression and temperature.However,the system of solid electrolyte(SE),as one of the most important components in SSLB,is usually plagued by clumsy ionic transport,leading to poor rate performance of the SSLBs.Herein,a unique perspective is proposed to re-examine the ion-transport behavior in lithium conductors by tracing Liþat multiscale,including microscopic,mesoscopic and macroscopic scales.The multi-scale ion-transport mechanisms and corresponding characterization techniques are analyzed in depth.Furthermore,some strategies of structure design to improve ion-transport kinetics at corresponding scales are elaborated systematically,involving the modulation of microscopic homogeneous structure,mesoscopic heterogeneous structure and macroscopic structures,etc.The proposed generalized rules for SEs are expected to construct a close link from mechanism-structure-characterization to high performances for SSLBs.
基金support from the National Key Technology R&D Program of China(2022YFB3504302,2022YFC3-901503)Natural Science Foundation and Overseas Talent Projects of Jiangxi Province(20232BAB214025,20232BCJ25044)Self-deployed Projects of Ganjiang Innovation Academy,Chinese Academy of Sciences(E355F003).
文摘Stabilizing the highly active RuO_(2) electrocatalyst for the oxygen evolution reaction(OER)is critical for the application of proton exchange membrane water electrolysis,but this remains challenging due to the inevitable over-oxidation of Ru in harsh oxidative environments.Herein,we describe constructing Ru-O-La asymmetric configurations into RuO_(2) via a facile sol-gel method to tailor electron redistribution and thereby eliminate the over-oxidation of Ru centers.Specifically,the as-prepared optimal La_(0.1)Ru_(0.9)O_(2) shows a low overpotential of 188 mV at 10 mA cm^(-2),a high mass activity of 251 A gRu^(-1) at 1.6 V vs.reversible hydrogen electrode(RHE),and a long-lasting durability of 63 h,far superior to the 8 h achieved by standard RuO_(2).Experiments and density functional theory calculations jointly reveal that the Ru-O-La asymmetric configuration could trigger electron redistribution in RuO_(2).More importantly,electron transfer from La to Ru via the Ru-O-La configuration could lead to increased electron density around Ru,thus preventing the over-oxidation of Ru.In addition,electron redistribution tunes the Ru 4d band center’s energy level,which optimizes the adsorption and desorption of oxygen intermediates.This work offers an effective strategy for regulating electronic structure to synergistically boost the activity and stability of RuO_(2)-based acidic OER electrocatalysts.
基金supported by the Key Research and Development Program of Hunan Province(2023GK2015)the Science and Technology Innovation Leader Program of Hunan Province(2022RC3049).
文摘Aqueous zinc-ion batteries(ZIBs)represent a promising solution for“beyond-lithium-ion”chemistries,but certain problems hinder their further development,especially when conventional aqueous electrolytes are involved.Hydrogel polymer electrolytes(HPEs)offer opportunities to circumvent these issues.This review aims to provide a fundamental understanding of how to design better HPEs for high-performing ZIBs,through critically analyzing the recent literature.Concerns regarding HPEs’mechanical,interfacial,and electrochemical characteristics are addressed,followed by in-depth insights into their underlying mechanisms.Possibilities for practical applications of HPEs are also discussed.
基金supported by the National Natural Science Foundation of China(No.22308322)Key R&D Program of Zhejiang(No.2024C03247)R&D Project of State Grid Corporation of China(No.5108-202218280A-2-439-XG,B311DS230005).
文摘As an important component in electrochemical energy conversion and storage systems,electrochemical reactors(ECRs)are widely used for commodity chemical synthesis,including electrolytic H_(2)production,NH_(3)synthesis,and high-value CO_(2)utilization.However,ECRs pose challenges related to low energy efficiency and selectivity due to the low solubility of their gaseous reactants,slow kinetics,and limitations in mass transfer.It is thus imperative to develop advanced high-pressure(HP)ECRs to address these issues.In this review,we start by presenting a comprehensive analysis of the fundamental mechanisms of HP ECRs.Then,we summarize the stateof-the-art HP ECR applications for water electrolysis,the N_(2)reduction reaction,and the CO_(2)reduction reaction.We also demonstrate that mathematical simulations are valuable tools for digital validation and guidance to accelerate the design of better reactors.Finally,we make recommendations on developing relevant specifications and standards for the industrial application of HP ECRs.
基金supported by the National Nature Science Foundation of China(No.22272205,No.22279164)Hunan Provincial Nature Science Foundation of China(No.2022JJ30685)+4 种基金Hunan Provincial Science and Technology Plan Project of China(No.2017TP1001)the Science and Technology Innovation Program of Hunan Province(2023RC3058)the Scientific and Technological Research Program of Chongqing Municipal Education Commission(No.KJZD-M202101401)Aid Program for Science and Technology Innovative Research Team in Higher Educational Institutions of Hunan Provincesupport from Science and Technology Innovation Team for Photovoltaic Power and Energy Storage Battery Key Technologies at General University in Hunan Province.D.S.acknowledges support from Young Elite Scientists Sponsorship Program by CAST(No.YESS20220432).
文摘There is an urgent need to develop innovative electrochemical energy storage devices that can offer high energy density,long lifespan,excellent rate capability,and improved security.For the electrochemical system,the electrode interphase,namely the cathode electrolyte interphase(CEI)and solid electrolyte interphase(SEI)play crucial roles in the operating mechanism,kinetics,and overall performance of the battery.However,the in-depth investigation of the unstable and complex electrode interphase is limited by the unavoidable air and moisture contact during the material transfer process and probable high-energy radiation damage in the characterization procedure.Recently,cryogenic techniques and in situ techniques have been developed and applied in the electrode interphase research to settle the radiation damage and air erosion,respectively.However,there has not been a special review that summarizes the relevant methods,so a systematic review is very important to accelerate the development.In this review,we summarize these two state-of-the-art methods,including their working principle,characterization process,advantages,and applications in electrode interphase analysis.And the integrative techniques,which are considered as the future development perspectives,are also discussed.This review can provide important directions for next-generation characterization techniques and strategies to effectively analyze the electrode interphase for advanced batteries.
基金supported by the National Natural Science Foundation of China(Grants No.22125903,22439003)National Key R&D Program of China(Grant 2022YFA1504100,2023YFB4005204)Doctoral Research Start-up Fund of Liaoning Province(No.2024-BSBA-36).
文摘Electrochemical water splitting is a pivotal technology in the large-scale production of green hydrogen for sus-tainable future energy provisions.Highly active,stable electrocatalysts have been extensively explored,but the majority suffer from low current densities and small sizes,rendering them unsuitable for industrial applications.Recently,however,the scalable production of electrocatalysts with high performance at large current densities has made tremendous progress.In this review,the current achievements in developing outstanding large elec-trocatalysts for high-current-density water electrolysis are described in detail.First,we introduce the funda-mentals of water electrolysis,the criteria for performance evaluation,and the requirements for producing electrocatalysts at scale under large current densities.Second,we summarize the key approaches for realizing large-sized electrocatalysts with excellent performance,including electrodeposition,corrosion engineering,and thermal treatment,as well as combinations of these methods.Finally,we offer perspectives on research challenges and propose directions for mass-producing high-performance electrocatalysts with large current densities for water electrolysis,to guide the further industrialization of water-electrolysis catalysts.
基金support by the Fundamental Research Funds for the National Natural Science Foundation of China(22379135)the Fundamental Research Funds for the Central Universities(WK2060000016)the Collaborative Innovation program of Hefei Science Center,CAS.
文摘Interfacial H_(2)release severely limits the reversibility and feasibility of aqueous Zn metal batteries for large-scale energy storage.Different from the conventional perception that H_(2)release mainly originates from the competition between hydrogen evolution reaction and Zn plating process,we herein surprisingly find that non-negligible H_(2)is also generated during stripping due to the accelerated chemical corrosion of the newly exposed Zn surface.To address this issue,we systematically screened the organic additives with different molecular structures and functional groups.Interestingly,a positive correlation between the adsorption strength of additives and the ability to inhibit the interfacial hydrogen release is found.Taking cysteamine(MEA)as a model additive,a gradient solid electrolyte interphase(SEI)is in situ formed at the Zn surface,acting as a chemical“barrier”to isolate interfacial water molecules from electrode surface consequently enable a higher Coulombic efficiency(>99.5%,4000 cycles)compared with that of MEA-free electrolyte(98.1%,189 cycles).This work provides a new understanding of the interfacial hydrogen release mechanism and the criteria for selecting additives for aqueous Zn metal anodes.
基金supported by the National Natural Science Foundation of China(No.22209183,22225902,U22A20436,52436005)the National key Research&Development Program of China(2022YFE0115900,2021YFA1501500)+2 种基金the CAS-Commonwealth Scientific and Industrial Research Organization(CSIRO)Joint Research Projects(121835KYSB20200039)Advanced Talents of Jiangsu University,China(Grant No.23JDG027)Natural Science Foundation of Fujian Province(2021J05100).
文摘The application of electrochemical technologies for chemical and fuel synthesis offers a significantly more eco-friendly method than traditional industrial practice.However,electrochemical synthesis in aqueous solutions often involves a sluggish oxygen evolution reaction(OER)at the anode,yielding products that are less economically viable and leading to inefficient energy use.This challenge has prompted extensive research into replacing the OER with fast,value-added oxidation reactions(OER alternatives)in electrolysis systems.In this review,we summarize the latest research progress in coupled electrochemical systems that integrate OER al-ternatives with reduction reactions,beyond hydrogen evolution reactions,in aqueous solutions to synthesize dual value-added products.After providing a general overview,we start by introducing two key factors:(i)electrolytic devices and(ii)advanced characterization techniques for mechanism investigation.The focus then shifts to catalysts developed so far and their corresponding catalytic mechanisms,and to the electrochemical performance of these hybrid electrolysis systems.Finally,we outline and discuss the challenges and prospects for these inte-grated electrochemical systems to offer insights into future research directions and applications.We envision that this review will provide a panorama of electrolysis systems for dual value-added products,thereby fostering the development of green synthesis with zero carbon emissions.
基金supported by the National Natural Science Foundation of China(Nos:22271018,22309012,and 22302013)the NSF of Guangdong Province(2023A1515010554).
文摘Building highly reactive electrocatalysts is of great significance for addressing the energy crisis and developing green energy.Electrocatalytic reactions occur at the interface of catalysts,where the physicochemical properties of the catalyst surface play a dominant role.In particular,the electron spin behavior on the catalyst surface has a decisive impact on the catalytic reaction process.This review initially introduces the definition of electron spin and methods for spin manipulation.Furthermore,we summarize the advanced characterization methods of electron spin.Then,we review the latest research advancements on the spin effect in the oxygen reduction reaction,oxygen evolution reaction,carbon dioxide reduction reaction,and nitrogen reduction reaction.The catalytic mechanisms of spin manipulation in these four reactions are thoroughly discussed.Finally,we propose key directions for the future development of spin effects in the field of electrocatalysis.This review contributes to a deeper understanding of the micromechanisms in electrocatalytic reactions.
基金support from National Natural Science Foundation of China,Grant Nos.52241701 and 52307249Shanghai Pujiang Program,Nos.22PJ1413100Fundamental Research Funds for the Central Universities at Tongji University,Nos.PA22120220426.
文摘It is anticipated that alkaline water electrolysis(AWE)technology will assume a significant role in the future energy sector,facilitating the integration of renewable energy and hydrogen production.Regrettably,the effi-ciency of AWE is not yet optimal.In particular,the inefficiency caused by bubbles at increased current density is often overlooked,necessitating a detailed understanding of the intricate relationship between bubble evolution and electrolytic reactions.This paper presents a comprehensive review of the fundamental theory and recent research on bubbles,and outlines the primary challenges and research directions for bubble dynamics in AWE.First,the theory of bubble nucleation,growth,and detachment is reviewed and summarized.Subsequently,the impact of bubbles on the diverse processes occurring during the electrolysis reaction is meticulously delineated and examined.The following section presents a thorough compilation and categorization of the methods employed to remove bubbles,with a detailed analysis of the strategies deployed to mitigate the impact of gas bubble traffic.Additionally,an in-depth exploration of the research methodology employed at each stage of the bubble evolution process is provided.Finally,the review concludes with a summary and outlook on the oppor-tunities and challenges associated with studying bubble dynamics in AWE,offering insights into innovative av-enues for efficient electrolytic hydrogen production.
文摘The authors regret an inadvertent error in Fig.3a where a methyl group was drawn as an ethyl group in the trimethyl phosphate(TMP)structure,resulting in ethyl dimethylphosphate.This unintentional oversight occurred during graphic preparation.A revised structure is provided here.
基金supported by the Natural Science Foundation of Fujian Province,China(2021J06001)National Natural Science Foundation of China(22372072)National Key Research and Development Program of China(2020YFB1505800).
文摘With issues of energy security and environmental crisis intensifying,we urgently need to develop energy storage systems with high energy density and high safety.Zinc–air batteries have attracted extensive attention for their energy density,safety,and low cost,but problems with the zinc anode—such as hydrogen evolution,corrosion,passivation,dendrite proliferation,and deformation—have led to zinc–air batteries with low Coulombic efficiency and short cycle life;these remain the key obstacles hindering the batteries’further development.In this review paper,we briefly describe the reaction mechanism of zinc–air batteries,then summarize the strategies for solving the key issues in zinc anodes.These approaches are divided into three aspects:structural designs for the zinc anode;interface engineering;and electrolyte selection and optimization.We finish by offering some suggestions for future research directions to improve the zinc anode in zinc–air batteries.
基金supported by the National Natural Science Foundation of China(Grant No.T2293692,21925404,22361132532,22021001)the Natural Science Foundation of Fujian Province(Grant No.2021J05193).
文摘The integration of surface plasmons with catalysis has opened a new frontier in the field of chemical energy conversion,offering unprecedented opportunities for enhancing reaction activity and selectivity.This review delves into the optical properties of plasmonic materials,the intricate mechanisms of plasmon-assisted chemical reactions(PACRs),and the fabrication of plasmonic catalysts,highlighting the significance of the structure–performance relationship.The mechanisms of PACRs are summarized to understand their synergistic contributions to reactions.The review further examines modern experimental strategies for characterizing surface plasmon resonance properties,including scanning probe microscope,in situ spectroscopy,and ultrafast laser pump-probe techniques,which provide real-time,dynamic insights into molecular interactions and structural changes with high spatial and temporal resolution.We conclude by outlining the challenges and future prospects for PACRs,emphasizing the need for innovative strategies to fully exploit the potential of PACRs for sustainable energy conversion and environmental remediation.
基金supported by the National Natural Science Foundation of China(Youth Program,No.22309209)the Key Research and Development Program of Hunan Province(Grant No.2023GK2015)+3 种基金the Leading Telant in Science and Technological Innovation Program of Hunan Province,China(No.2022RC3049)the Tianshan Innovation Team Program of Xinjiang,China(No.2024D14001)the Natural Science Foundation of Hunan Province China(Grant No.2023JJ40709)This project was also supported by the State Key Laboratory of Powder Metallurgy,Central South University.
文摘Integrating single atoms and clusters into a unified catalytic system represents a novel strategy for enhancing catalytic performance.Compared to single-atom catalysts,those incorporating both single atoms and clusters exhibit superior catalytic activity.However,the co-construction of these systems and the mechanisms of their catalytic efficacy remain challenging and poorly understood.In this study,we synthesized a Mn–N–C catalyst featuring MnY clusters and Mn single atoms via a straightforward two-step sintering method.Y doping facilitated the formation of Mn clusters and optimized the d-band center of Mn through a unique synergy effect,thereby reducing energy barriers and enhancing the reaction kinetics.Additionally,the electron-donating ability of Y single atoms promoted the formation of unsaturated Mn–N_(₃)coordination structures,resulting in excellent oxygen reduction reaction(ORR)performance.Consequently,the MnY/NC catalyst demonstrated a half-wave potential(E_(₁/₂))of 0.90 V and maintained stability in 0.1 M KOH,outperforming both Mn/NC and Pt/C.This work underscores the potential of rare earth metal doping in transition metals to create stable single-atom and cluster systems,effectively leveraging their synergy effect for superior catalytic performance and validating the concept of the“remote synergy effect”in heterogeneous catalysis.
基金supported by the National Natural Science Foundation of China(52373087,51973235,52173091,22208331 and 62274050)Program for Leading Talents of National Ethnic Affairs Commission of China(MZR21001)+2 种基金Hubei Provincial Natural Science Foundation of China(2021CFA022)Wuhan Science and Technology Bureau(2020010601012198)Zhejiang Provincial Natural Science Foundation of China under Grant No.LZ21E020002.
文摘Bismuth vanadate(BiVO_(4))is a promising photoanode material for photoelectrochemical(PEC)water oxidation.However,its performance is greatly hindered by poor bulk and interfacial charge transfer.Herein,to address this issue,iron doped vanadyl phosphate(Fe:VOPO_(4))was grafted on molybdenum doped BiVO_(4)(Mo:BiVO_(4))for significantly enhancing charge transfer and oxygen evolution kinetics simultaneously.Consequently,the resultant Fe:VOPO_(4)/Mo:BVO_(4) photoanode exhibits a remarkable photocurrent density of 6.59 mA cm^(-2) at 1.23 V versus the reversible hydrogen electrode(VRHE)under AM 1.5G illumination,over approximately 5.5 times as high as that of pristine BiVO_(4).Systematic studies have demonstrated that the hopping activation energy of small polarons is significantly reduced due to the Mo doping,resulting in accelerated bulk charge transfer.More importantly,the deposition of Fe:VOPO_(4) promotes the interfacial charge transfer between Mo:BiVO_(4) and Fe:VOPO_(4) via the construction of V-O-V and P-O bonds,in addition to facilitating water splitting kinetics.This work provides a general strategy for optimizing charge transfer process,especially at the interface between photoanodes and cocatalysts.
基金supported by the National Key Research and Development Program of China(2023YFB2503600)Yunnan Major Scientific and Technological Projects(grant NO.202402AF080004)+1 种基金the National Natural Science Foundation of China(22279089)the Municipal Key R&D Program of Ningbo(2023Z109).
文摘Black phosphorus(BP)anode with high capacity(2596 mAh g^(-1))and suitable lithiation potential(0.7 V vs.Li^(+)/Li)is an ideal candidate for high-energy-density and high-safety lithium-ion batteries,however,the practical implementation is greatly limited by its slow reaction kinetics and huge volume expansion.Here,inspired by nature,liquid metal(LM)is explored as a self-heal agent,which can well stabilize the BP anode through buffering the volumetric expansion and re-activating“dead P and Li x P”.Moreover,LM also acts as a good catalyst,which can adjust Li ion concentration and reduce the activation energy of delithiation reaction,thus prolonging the cycling life.Therefore,the LM modified BP/graphite(G)composite delivers an excellent high-rate performance of 1123 mAh g^(-1)at 4 C with 80.0%capacity retention after 200 cycles,a superior wide-temperature performance of 1547.5 mAh g^(-1)and 569.0 mAh g^(-1)at 50℃and-20℃,respectively.
基金supported by the National Natural Science Foundation of China(Grant No.62105238)。
文摘Full-body avatar reconstruction offers users immersive and interactive experiences in virtual space,which are crucial for the advancement of metaverse applications.However,traditional hardware solutions,reliant on optical cameras or inertial sensors,are hampered by privacy concerns,spatial limitations,high costs,and calibration challenges.Here,we propose AI-enabled smart clothing that seamlessly integrates triboelectric strain-sensing fibers(TSSFs)and AI algorithms with commercial fitness suits to achieve precise dynamic 3D reconstruction of body movement.TSSFs enable the dynamic capture of body postures and excel in sensitivity,linearity,and strain range,while maintaining mechanical stability,temperature resilience,and washability.The integrated algorithms accurately decouple posture signals—distinguishing between similar postures with the 1D-CNN algorithm,compensating for body-shape differences via a calibration algorithm,and determining spatial elements for avatar reconstruction using a decision-tree algorithm.Finally,leveraging Unity-3D,we achieve ultra-accurate dynamic 3D avatars with a joint angle error of<3.63°and demonstrate their effectiveness using VR fitness and enter-tainment applications,showing how they can offer users standardized yet engaging experiences.
基金supported by National Natural Science Foundation of China(Grant No.52002094,22479037)Guangdong Basic and Applied Basic Research Foundation(Grant No.2019A1515110756)+2 种基金Shenzhen Science and Technology Program(Grant No.JCYJ20210324121411031,JSGG202108021253804014,RCBS20210706092218040)the Shenzhen Steady Support Plan(GXWD20221030205923001,GXWD20201230155427003-20200824103000001)State Key Laboratory of Precision Welding&Joining of Materials and Structures(Grant Nos.24-Z-17,24-T-08).
文摘The Li-O_(2) battery(LOB)has attracted growing interest,including for its great potential in next-generation energy storage systems due to its extremely high theoretical specific capacity.However,a series of challenges have seriously hindered LOB development,such as sluggish kinetics during the oxygen reduction and oxygen evolution reactions(ORR/OER)at the cathode,the formation of lithium dendrites,and undesirable corrosion at the lithium metal anode.Herein,we propose a strategy based on the ultra-low loading of atomic Ni catalysts to simultaneously boost the ORR/OER at the cathode while stabilizing the Li metal anode.The resultant LOB delivers a superior discharge capacity(>16,000 mAh g^(-1)),excellent long-term cycling stability(>200 cycles),and enhanced high rate capability(>300 cycles@500 mA g^(-1)).The working mechanisms of these atomic Ni catalysts are revealed through carefully designed in situ experiments and theoretical calculations.This work provides a novel research paradigm for designing high-performance LOBs that are useable in practical applications.
基金supported by the National Key R&D Program of China(2021YFB2402002)Beijing Natural Science Foundation(Grant No.L223013)the National Natural Science Foundation of China(Grant No.52272359 and 52376167).
文摘Accelerated and accurate degradation diagnosis is imperative for the management and reutilization of commercial lithium-ion batteries in the upcoming TWh era.Different from traditional methods,this work proposes a hybrid framework for rapid and accurate degradation diagnosis at the electrode level combining both deep learning,which is used to rapidly and robustly predict polarization-free incremental capacity analysis(ICA)curves in minutes,and physical modeling,which is used to quantitatively reveal the electrode-level degradation modes by decoupling them from the ICA curves.Only measured charging current and voltage signals are used.Results demonstrates that 11 points collected at any starting state-of-charge(SOC)in a minimum of 2.5 minutes are sufficient to obtain reliable ICA curves with a mean root mean square error(RMSE)of 0.2774 Ah/V.Accordingly,battery status can be accurately elevated based on their degradation at both macro and electrode levels.Through transfer learning,such a method can also be adapted to different battery chemistries,indicating the enticing potential for wide applications.
